Pierre-Michel Adam

Enhancement and Quenching Regimes in Metal−Semiconductor Hybrid Optical Nanosources

We report on the emission of hybrid nanosources composed of gold nanoparticles coupled with quantum dots. The emission relies on energy transfer from the quantum dots to gold nanoparticles which could be de-excited through radiative plasmon relaxation. The dependence of the emission efficiency is studied systematically as a function of the size of gold nanoparticles and interdistance between gold nanoparticles and quantum dots. We demonstrate a size-dependent transition between quenching and enhancement and a nonradiative energy transfer from the quantum dots to the gold nanoparticles.

Short Range Plasmon Resonators Probed by Photoemission Electron Microscopy

Short range surface plasmon resonators are investigated at the nanometer scale. Gold nanorods (30 nm in diameter) were microfabricated and probed by photoemission electron microscopy under direct laser light excitation. Resonances presenting various numbers of lobes occur for specific rod lengths. A simple analytical model shows that the successive resonant lengths differ by a multiple of one-half of the wavelength of the supported short-range surface plasmon polariton.

Role of surface plasmon in second harmonic generation from gold nanorods

The role of surface plasmon in second harmonic generation from arrays of gold nanorod particles excited by femtosecond laser pulses is investigated as a function of incident light polarization and irradiation wavelength. In addition to photoluminescence, a peak of second harmonic is observed and is found to depend on the polarization and wavelength of the fundamental frequency laser beam. In particular, the authors found similarities between extinction spectra of the nanoparticles and spectra of emmitted second harmonic. This behavior can be explained by resonant excitation of localized surface plasmon resonances.

Optimization of SERS-active substrates for near-field Raman spectroscopy

As a first step towards near-field Raman, we chose to study surface enhanced Raman scattering (SERS)-active substrates to cope with the weakness of Raman scattering (small cross-section and low concentration). We concentrated our work on localized surface plasmon (LSP) since they turned out to play a great part in SERS and we put forward the relation between LSP resonance and Raman enhancement. Roughness of our samples is controlled either by annealing process or electron-beam lithography (EBL); this latter technique proved to best suit to our study. Substrates are characterized by extinction spectroscopy which determines the LSP resonance and then Raman spectrum of a probe molecule, trans-1,2-bis(4-pyridyl)ethylene (BPE) is recorded. We show that maximum of enhancement is obtained when the LSP resonance is red-shifted (50 nm) compared to the excitation laser line (632.8 nm).

Near-field second-harmonic generation in single gold nanoparticles

Second-harmonic generation from single gold elliptical nanoparticles is experimentally investigated by a nonlinear scanning near-field optical microscope (SNOM). The near-field nonlinear response is found to be directly related to local surface plasmon resonances and to particle morphology. The combined analysis of linear and second-harmonic SNOM images provides discrimination among different light extinction particle behaviors, not achievable just with linear techniques. The polarization state of the emitted second harmonic is also investigated, providing experimental evidence of second-harmonic particle emission modes peculiar to near-field excitation.

Nonresonant Surface-Enhanced Raman Scattering of ZnO Quantum Dots with Au and Ag Nanoparticles

Pronounced 10(4)-fold enhancement of Raman scattering has been obtained for ZnO nanocrystals on substrates coated with 50 nm Ag nanoparticles under nonresonant excitation with a commercial red-emitting laser. This makes feasible beyond 10(-18) mole detection of ZnO nanocrystals with a commercial setup using a 0.1 mW continuous wave laser and can be purposefully used in analytical applications where conjugated nanocrystals serve as Raman markers. For Au-coated surfaces the enhancement is much lower and the heating effects in the course of Raman experiments are pronounced.

Influence of tip modulation on image formation in scanning near-field optical microscopy

Modulation of the probe height in a scanning near-field optical microscope (SNOM) is a technique that is commonly used for both distance control and separation of the near-field signal from a background. Detection of higher harmonic modulated signals has also been used to obtain an improvement in resolution, the elimination of background, or artifacts in the signal. This article presents a theoretical model for the effects induced in SNOM images by modulation of the probe. It is shown that probe modulation introduces a spatial filter into the image, generally suppressing propagating field components and enhancing the strength of evanescent field components. A simple example of detection of a single evanescent field above a prism is studied in some detail, and a complicated dependence on modulation parameters and waveform is shown. Some aspects of the application of this theory in a general experimental situation are discussed. Simulated images are displayed to explicitly show the effects of varying modula...

Reversible strong coupling in silver nanoparticle arrays using photochromic molecules.

In this Letter, we demonstrate a reversible strong coupling regime between a dipolar surface plasmon resonance and a molecular excited state. This reversible state is experimentally observed on silver nanoparticle arrays embedded in a polymer film containing photochromic molecules. Extinction measurements reveal a clear Rabi splitting of 294 meV, corresponding to ~13% of the molecular transition energy. We derived an analytical model to confirm our observations, and we emphasize the importance of spectrally matching the polymer absorption with the plasmonic resonance to observe coupled states. Finally, the reversibility of this coupling is illustrated by cycling the photochromic molecules between their two isomeric forms.

Biological and chemical gold nanosensors based on localized surface plasmon resonance

In this paper, we discuss the performances of gold nanosensors based on Localized Surface Plasmon Resonance (LSPR) designed by Electron Beam Lithography (EBL) in the context of biological and chemical sensing. We demonstrate the sensitivity of our gold nanosensors by studying the influence of the concentration of 11-mercaptoundecanoic acid (MUA) on the shift of LSPR wavelength. Additionally, to study the selectivity of our nanosensors, the system Biotin/Streptavidin was used to detect very weak concentration of biomolecules. These results represent new steps for applications in chemical research and medical diagnostics.

Analysis of the influence of the tip vibration in the formation of images in apertureless scanning near-field optical microscopy

The theoretical influence of the vertical vibration of the tip is investigated to calculate the images of a quartz grating in an apertureless scanning near-field optical microscope configuration, a realistic model is used for the simulation of the lock-in detection. It is shown that the output signal issued from the lock-in detection cannot be simply approximated by a mere difference between the intensities of the field between the top and bottom positions of the tip oscillation. Several modes of the lock-in detection, amplitude and phase, X and Y channels, at the fundamental frequency or for the following harmonics, though all leading to images containing high spatial frequencies of the grating, show significant differences that can induce misinterpretations in specific cases.